IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-49973-9.html
   My bibliography  Save this article

Unraveling the energy storage mechanism in graphene-based nonaqueous electrochemical capacitors by gap-enhanced Raman spectroscopy

Author

Listed:
  • Xiao-Ting Yin

    (Xiamen University)

  • En-Ming You

    (Jimei University)

  • Ru-Yu Zhou

    (Xiamen University)

  • Li-Hong Zhu

    (Xiamen University)

  • Wei-Wei Wang

    (Xiamen University)

  • Kai-Xuan Li

    (Xiamen University)

  • De-Yin Wu

    (Xiamen University)

  • Yu Gu

    (Xiamen University)

  • Jian-Feng Li

    (Xiamen University)

  • Bing-Wei Mao

    (Xiamen University)

  • Jia-Wei Yan

    (Xiamen University)

Abstract

Graphene has been extensively utilized as an electrode material for nonaqueous electrochemical capacitors. However, a comprehensive understanding of the charging mechanism and ion arrangement at the graphene/electrolyte interface remain elusive. Herein, a gap-enhanced Raman spectroscopic strategy is designed to characterize the dynamic interfacial process of graphene with an adjustable number of layers, which is based on synergistic enhancement of localized surface plasmons from shell-isolated nanoparticles and a metal substrate. By employing such a strategy combined with complementary characterization techniques, we study the potential-dependent configuration of adsorbed ions and capacitance curves for graphene based on the number of layers. As the number of layers increases, the properties of graphene transform from a metalloid nature to graphite-like behavior. The charging mechanism shifts from co-ion desorption in single-layer graphene to ion exchange domination in few-layer graphene. The increase in area specific capacitance from 64 to 145 µF cm–2 is attributed to the influence on ion packing, thereby impacting the electrochemical performance. Furthermore, the potential-dependent coordination structure of lithium bis(fluorosulfonyl) imide in tetraglyme ([Li(G4)][FSI]) at graphene/electrolyte interface is revealed. This work adds to the understanding of graphene interfaces with distinct properties, offering insights for optimization of electrochemical capacitors.

Suggested Citation

  • Xiao-Ting Yin & En-Ming You & Ru-Yu Zhou & Li-Hong Zhu & Wei-Wei Wang & Kai-Xuan Li & De-Yin Wu & Yu Gu & Jian-Feng Li & Bing-Wei Mao & Jia-Wei Yan, 2024. "Unraveling the energy storage mechanism in graphene-based nonaqueous electrochemical capacitors by gap-enhanced Raman spectroscopy," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-49973-9
    DOI: 10.1038/s41467-024-49973-9
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-49973-9
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-024-49973-9?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. Alexander C. Forse & John M. Griffin & Céline Merlet & Javier Carretero-Gonzalez & Abdul-Rahman O. Raji & Nicole M. Trease & Clare P. Grey, 2017. "Direct observation of ion dynamics in supercapacitor electrodes using in situ diffusion NMR spectroscopy," Nature Energy, Nature, vol. 2(3), pages 1-7, March.
    2. Yu Gu & En-Ming You & Jian-De Lin & Jun-Hao Wang & Si-Heng Luo & Ru-Yu Zhou & Chen-Jie Zhang & Jian-Lin Yao & Hui-Yang Li & Gen Li & Wei-Wei Wang & Yu Qiao & Jia-Wei Yan & De-Yin Wu & Guo-Kun Liu & Li, 2023. "Resolving nanostructure and chemistry of solid-electrolyte interphase on lithium anodes by depth-sensitive plasmon-enhanced Raman spectroscopy," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    3. Jian Feng Li & Yi Fan Huang & Yong Ding & Zhi Lin Yang & Song Bo Li & Xiao Shun Zhou & Feng Ru Fan & Wei Zhang & Zhi You Zhou & De Yin Wu & Bin Ren & Zhong Lin Wang & Zhong Qun Tian, 2010. "Shell-isolated nanoparticle-enhanced Raman spectroscopy," Nature, Nature, vol. 464(7287), pages 392-395, March.
    4. K. S. Novoselov & V. I. Fal′ko & L. Colombo & P. R. Gellert & M. G. Schwab & K. Kim, 2012. "A roadmap for graphene," Nature, Nature, vol. 490(7419), pages 192-200, October.
    5. Sheng Bi & Runxi Wang & Shuai Liu & Jiawei Yan & Bingwei Mao & Alexei A. Kornyshev & Guang Feng, 2018. "Minimizing the electrosorption of water from humid ionic liquids on electrodes," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
    6. Yao-Hui Wang & Shisheng Zheng & Wei-Min Yang & Ru-Yu Zhou & Quan-Feng He & Petar Radjenovic & Jin-Chao Dong & Shunning Li & Jiaxin Zheng & Zhi-Lin Yang & Gary Attard & Feng Pan & Zhong-Qun Tian & Jian, 2021. "In situ Raman spectroscopy reveals the structure and dissociation of interfacial water," Nature, Nature, vol. 600(7887), pages 81-85, December.
    7. Jack Fawdon & Johannes Ihli & Fabio La Mantia & Mauro Pasta, 2021. "Characterising lithium-ion electrolytes via operando Raman microspectroscopy," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Chao-Yu Li & Ming Chen & Shuai Liu & Xinyao Lu & Jinhui Meng & Jiawei Yan & Héctor D. Abruña & Guang Feng & Tianquan Lian, 2022. "Unconventional interfacial water structure of highly concentrated aqueous electrolytes at negative electrode polarizations," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    2. Ling Tong & Zhou Yu & Yi-Jing Gao & Xiao-Chong Li & Ju-Fang Zheng & Yong Shao & Ya-Hao Wang & Xiao-Shun Zhou, 2023. "Local cation-tuned reversible single-molecule switch in electric double layer," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    3. Hao Shi & Tanyuan Wang & Jianyun Liu & Weiwei Chen & Shenzhou Li & Jiashun Liang & Shuxia Liu & Xuan Liu & Zhao Cai & Chao Wang & Dong Su & Yunhui Huang & Lior Elbaz & Qing Li, 2023. "A sodium-ion-conducted asymmetric electrolyzer to lower the operation voltage for direct seawater electrolysis," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    4. Zhi Chang & Huijun Yang & Xingyu Zhu & Ping He & Haoshen Zhou, 2022. "A stable quasi-solid electrolyte improves the safe operation of highly efficient lithium-metal pouch cells in harsh environments," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    5. Cheng Chi & Gongze Liu & Meng An & Yufeng Zhang & Dongxing Song & Xin Qi & Chunyu Zhao & Zequn Wang & Yanzheng Du & Zizhen Lin & Yang Lu & He Huang & Yang Li & Chongjia Lin & Weigang Ma & Baoling Huan, 2023. "Reversible bipolar thermopower of ionic thermoelectric polymer composite for cyclic energy generation," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    6. Choudhary, Ram Bilash & Ansari, Sarfaraz & Majumder, Mandira, 2021. "Recent advances on redox active composites of metal-organic framework and conducting polymers as pseudocapacitor electrode material," Renewable and Sustainable Energy Reviews, Elsevier, vol. 145(C).
    7. Dehui Zhang & Zhen Xu & Gong Cheng & Zhe Liu & Audrey Rose Gutierrez & Wenzhe Zang & Theodore B. Norris & Zhaohui Zhong, 2022. "Strongly enhanced THz generation enabled by a graphene hot-carrier fast lane," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    8. Li, Yong & Song, Jian & Yang, Jie, 2015. "Graphene models and nano-scale characterization technologies for fuel cell vehicle electrodes," Renewable and Sustainable Energy Reviews, Elsevier, vol. 42(C), pages 66-77.
    9. Zhi Chang & Huijun Yang & Anqiang Pan & Ping He & Haoshen Zhou, 2022. "An improved 9 micron thick separator for a 350 Wh/kg lithium metal rechargeable pouch cell," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    10. Jin Ming Wang & Qin Yao Zhu & Jeong Heon Lee & Tae Gyun Woo & Yue Xing Zhang & Woo-Dong Jang & Tae Kyu Kim, 2023. "Asymmetric gradient orbital interaction of hetero-diatomic active sites for promoting C − C coupling," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    11. Ling Ding & Tianqi Xu & Jiawen Zhang & Jinpeng Ji & Zhaotao Song & Yanan Zhang & Yijun Xu & Tong Liu & Yang Liu & Zihan Zhang & Wenbin Gong & Yunong Wang & Zhenzhong Shi & Renzhi Ma & Jianxin Geng & H, 2024. "Covalently bridging graphene edges for improving mechanical and electrical properties of fibers," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    12. Chongyang Tang & Cong Wei & Yanyan Fang & Bo Liu & Xianyin Song & Zenan Bian & Xuanwei Yin & Hongbo Wang & Zhaohui Liu & Gongming Wang & Xiangheng Xiao & Xiangfeng Duan, 2024. "Electrocatalytic hydrogenation of acetonitrile to ethylamine in acid," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    13. Daniel Rueda-García & María del Rocío Rodríguez-Laguna & Emigdio Chávez-Angel & Deepak P. Dubal & Zahilia Cabán-Huertas & Raúl Benages-Vilau & Pedro Gómez-Romero, 2019. "From Thermal to Electroactive Graphene Nanofluids," Energies, MDPI, vol. 12(23), pages 1-11, November.
    14. Di Blasi, O. & Briguglio, N. & Busacca, C. & Ferraro, M. & Antonucci, V. & Di Blasi, A., 2015. "Electrochemical investigation of thermically treated graphene oxides as electrode materials for vanadium redox flow battery," Applied Energy, Elsevier, vol. 147(C), pages 74-81.
    15. Shobhan Dhir & Ben Jagger & Alen Maguire & Mauro Pasta, 2023. "Fundamental investigations on the ionic transport and thermodynamic properties of non-aqueous potassium-ion electrolytes," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    16. Le Cheng & Chi Shun Yeung & Libei Huang & Ge Ye & Jie Yan & Wanpeng Li & Chunki Yiu & Fu-Rong Chen & Hanchen Shen & Ben Zhong Tang & Yang Ren & Xinge Yu & Ruquan Ye, 2024. "Flash healing of laser-induced graphene," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    17. Xiaoxia Chang & Sudarshan Vijay & Yaran Zhao & Nicholas J. Oliveira & Karen Chan & Bingjun Xu, 2022. "Understanding the complementarities of surface-enhanced infrared and Raman spectroscopies in CO adsorption and electrochemical reduction," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    18. Qian Zhang & Bo Gao & Ling Zhang & Xiaopeng Liu & Jixiang Cui & Yijun Cao & Hongbo Zeng & Qun Xu & Xinwei Cui & Lei Jiang, 2023. "Anomalous water molecular gating from atomic-scale graphene capillaries for precise and ultrafast molecular sieving," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    19. Christos Kalantaridis, 2019. "Is university ownership a sub-optimal property rights regime for commercialisation? Information conditions and entrepreneurship in Greater Manchester, England," The Journal of Technology Transfer, Springer, vol. 44(1), pages 231-249, February.
    20. Xiaoju Yang & Chao Rong & Li Zhang & Zhenkun Ye & Zhiming Wei & Chengdi Huang & Qiao Zhang & Qing Yuan & Yueming Zhai & Fu-Zhen Xuan & Bingjun Xu & Bowei Zhang & Xuan Yang, 2024. "Mechanistic insights into C-C coupling in electrochemical CO reduction using gold superlattices," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-49973-9. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.